Investigations of Bio-Organic Hybrid Assemblies

Henna Rosilo

Investigations of Bio-Organic Hybrid Assemblies

Julkaisun otsikon käännös: Bio-orgaanisten hybridirakenteiden tutkimuksia

Henna Rosilo

Teknillisen fysiikan laitos

Tutkimustuotos: Doctoral Thesis › Collection of Articles

Abstrakti

Supramolekyylikemian, itsejärjestymisen ja luontoa imitoivien lähestymistapojen kehittyminen on mahdollistanut hyvin määriteltyjen, hierarkkisten ja funktionaalisten nanomateriaalien valmistuksen. Luonnossa lähes täydelliset makromolekyylit ja järjestyneet materiaalit muodostuvat yksinkertaisista rakenneosista miedoissa olosuhteissa. Materiaalitutkimukseen nämä biomateriaalit tuovat uutta täsmällisyyttä, monimuotoisuutta ja toiminnallisuutta. Väitöskirjassa osoitetaan, kuinka biologiset ja synteettiset orgaaniset materiaalit voidaan yhdistää hybridimateriaaleiksi hyödyttäen lääketiedettä ja komposiittitutkimusta. Julkaisussa I valmistettiin monivalentteja, pelkistämällä hajotettavia disulfidisidoksia sisältäviä dendroneita ja tutkittiin niiden kykyä sitoa DNA:ta ionisilla vuorovaikutuksilla ja vapauttaa se ulkoisen signaalin avulla. Dendronien affiniteetti DNA:ta kohtaan riippui niiden valenssista, ja pelkistys vapautti DNA:n nopeasti. Menetelmä voi tehostaa geeniterapiaa, jossa solujen pelkistävä ympäristö hajottaa DNA-dendroni –kompleksit. Julkaisussa II pelkistettäviä ja valon avulla hajotettavia dendroneita käytettiin DNA-origamien muodostumisen hallintaan. Origamien rakenneosien sitominen dendroneilla esti niiden itsejärjestymisen, joka voitiin käynnistää hajottamalla dendronit ulkoisilla signaaleilla. Lisäksi dendronit kokosivat ja vapauttivat hallitusti kokonaisia origameja. Julkaisu III tutki anionisten, ikosaedrin muotoisten virusten ja amfifiilisten Janus-dendrimeerien järjestymistä. Dendrimeerien rakenteiden ja elektrolyyttikonsentraatioiden säätely tuotti superhiloja pintakeskisellä kuutiollisella kiderakenteella. Luonnossa esiintyviä inkluusiokappaleita muistuttavat kiteet voivat edesauttaa niiden tutkimusta. Julkaisussa IV kationista polymeeriä oksastettiin sauvamaisten selluloosan nanokiteiden pinnalta. Geeninsiirtoa tehostavia peptidikuituja muistuttavat kationiset selluloosakiteet sitoivat anionisia viruksia tehokkaasti ja mahdollistivat niiden eristämisen liuoksesta. Komplekseista virukset voidaan siirtää jatkotutkimuksiin tai vapauttaa nostamalla elektrolyyttikonsentraatiota. Julkaisussa V selluloosan nanokiteisiin liitettiin hydrofobisia, ristisilloitettavia alkyyliketjuja, ja niillä vahvistettiin synteettistä kumia. Nanokiteet järjestyivät kosteutta hylkivissä komposiiteissa suurissa pitoisuuksissa biomimeettisiksi orientoituneiksi ja hierarkkisiksi kerrosrakenteiksi. Nanokiteiden määrän kasvaessa komposiittien jännitys-venymä –käyrä muuttui äkillisesti kumimaisesta lähes lineaariseksi, kimmokertoimen kasvaessa lähes kaksi kertaluokkaa.

Julkaisun otsikon käännös	Bio-orgaanisten hybridirakenteiden tutkimuksia
Alkuperäiskieli	Englanti
Pätevyys	Tohtorintutkinto
Myöntävä instituutio	Aalto-yliopisto
Valvoja/neuvonantaja	Ikkala, Olli, Vastuuprofessori Kostiainen, Mauri, Ohjaaja
Kustantaja	Aalto University
Painoksen ISBN	978-952-60-5971-6
Sähköinen ISBN	978-952-60-5972-3
Tila	Julkaistu - 2014
OKM-julkaisutyyppi	G5 Artikkeliväitöskirja

Tutkimusalat

biohybridimateriaali
virus
nanokiteinen selluloosa
dendroni
dendrimeeri
komposiitti

Pääsy asiakirjaan

http://urn.fi/URN:ISBN:978-952-60-5972-3

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@phdthesis{71946febeb774dbd9ba29c165f8693fe,

title = "Investigations of Bio-Organic Hybrid Assemblies",

abstract = "The advances of supramolecular chemistry, bottom-up fabrication and bioinspired approaches have opened pathways to well-defined, hierarchical and functional materials at nanometer scale. Biological systems master the fabrication of near-perfect macromolecules and organized bulk materials from simple components under mild conditions. For self-assembly and material applications these biomaterials offer precision, diversity and functionality. This thesis demonstrates how biological and synthetic organic materials can be combined into bio-organic hybrid assemblies to promote biomedical and composite applications. In publication I multivalent, low-molecular-weight dendrons with cleavable disulfide bonds were synthesized and used for the electrostatic binding and triggered release of DNA. The dendrons bound DNA in a generation-dependent fashion and reduction of the disulfide bonds rapidly liberated the DNA. Degradable multivalent binding has been shown to enhance gene delivery, as the reducing cytosolic environment induces the release of DNA. In publication II the reducible dendrons were combined with photocleavable dendrons for the controlled formation of nanoscale DNA origamis. Binding of the origami constituents prevented their self-assembly into origamis, which was subsequently initiated by externally triggered degradation of the dendrons. Publication III studied the co-assembly of anionic icosahedral viruses and amphiphilic Janus dendrimers. Tuning of the dendrimer structures and the electrolyte concentration provided superlattices with a face-centered cubic unit cell. The assemblies resembled natural viral inclusion bodies, and provide means for studying their self-assembly processes. In publication IV rod-like cellulose nanocrystals (CNC) were grafted with a cationic polymer. The cationic CNCs efficiently assembled the anionic icosahedral viruses. Additionally, the CNCs enabled the concentration and extraction of the viruses from solution. The assemblies can be further transferred to biomedical applications and allow the recovery of viruses via electrolyte-gated release. In publication V the CNCs were functionalized with cross-linkable alkyl chains and used for the reinforcement of a synthetic rubber. The moisture-repellent composites showed a hierarchical structure, where the CNCs assembled into ordered biomimetic structures at high weight fractions. Simultaneously the stress-strain behavior abruptly changed from nonlinear rubbery to almost linear with increasing CNC fraction, while the tensile modulus increased by almost two orders of magnitude.",

keywords = "biohybrid material, assembly, DNA, virus, cellulose nanocrystal, dendron, dendrimer, composite, biohybridimateriaali, virus, nanokiteinen selluloosa, dendroni, dendrimeeri, komposiitti, biohybrid material, assembly, DNA, virus, cellulose nanocrystal, dendron, dendrimer, composite",

author = "Henna Rosilo",

year = "2014",

language = "English",

isbn = "978-952-60-5971-6",

series = "Aalto University publication series DOCTORAL DISSERTATIONS",

publisher = "Aalto University",

number = "188",

address = "Finland",

school = "Aalto University",

}

TY - BOOK

T1 - Investigations of Bio-Organic Hybrid Assemblies

AU - Rosilo, Henna

PY - 2014

Y1 - 2014

N2 - The advances of supramolecular chemistry, bottom-up fabrication and bioinspired approaches have opened pathways to well-defined, hierarchical and functional materials at nanometer scale. Biological systems master the fabrication of near-perfect macromolecules and organized bulk materials from simple components under mild conditions. For self-assembly and material applications these biomaterials offer precision, diversity and functionality. This thesis demonstrates how biological and synthetic organic materials can be combined into bio-organic hybrid assemblies to promote biomedical and composite applications. In publication I multivalent, low-molecular-weight dendrons with cleavable disulfide bonds were synthesized and used for the electrostatic binding and triggered release of DNA. The dendrons bound DNA in a generation-dependent fashion and reduction of the disulfide bonds rapidly liberated the DNA. Degradable multivalent binding has been shown to enhance gene delivery, as the reducing cytosolic environment induces the release of DNA. In publication II the reducible dendrons were combined with photocleavable dendrons for the controlled formation of nanoscale DNA origamis. Binding of the origami constituents prevented their self-assembly into origamis, which was subsequently initiated by externally triggered degradation of the dendrons. Publication III studied the co-assembly of anionic icosahedral viruses and amphiphilic Janus dendrimers. Tuning of the dendrimer structures and the electrolyte concentration provided superlattices with a face-centered cubic unit cell. The assemblies resembled natural viral inclusion bodies, and provide means for studying their self-assembly processes. In publication IV rod-like cellulose nanocrystals (CNC) were grafted with a cationic polymer. The cationic CNCs efficiently assembled the anionic icosahedral viruses. Additionally, the CNCs enabled the concentration and extraction of the viruses from solution. The assemblies can be further transferred to biomedical applications and allow the recovery of viruses via electrolyte-gated release. In publication V the CNCs were functionalized with cross-linkable alkyl chains and used for the reinforcement of a synthetic rubber. The moisture-repellent composites showed a hierarchical structure, where the CNCs assembled into ordered biomimetic structures at high weight fractions. Simultaneously the stress-strain behavior abruptly changed from nonlinear rubbery to almost linear with increasing CNC fraction, while the tensile modulus increased by almost two orders of magnitude.

AB - The advances of supramolecular chemistry, bottom-up fabrication and bioinspired approaches have opened pathways to well-defined, hierarchical and functional materials at nanometer scale. Biological systems master the fabrication of near-perfect macromolecules and organized bulk materials from simple components under mild conditions. For self-assembly and material applications these biomaterials offer precision, diversity and functionality. This thesis demonstrates how biological and synthetic organic materials can be combined into bio-organic hybrid assemblies to promote biomedical and composite applications. In publication I multivalent, low-molecular-weight dendrons with cleavable disulfide bonds were synthesized and used for the electrostatic binding and triggered release of DNA. The dendrons bound DNA in a generation-dependent fashion and reduction of the disulfide bonds rapidly liberated the DNA. Degradable multivalent binding has been shown to enhance gene delivery, as the reducing cytosolic environment induces the release of DNA. In publication II the reducible dendrons were combined with photocleavable dendrons for the controlled formation of nanoscale DNA origamis. Binding of the origami constituents prevented their self-assembly into origamis, which was subsequently initiated by externally triggered degradation of the dendrons. Publication III studied the co-assembly of anionic icosahedral viruses and amphiphilic Janus dendrimers. Tuning of the dendrimer structures and the electrolyte concentration provided superlattices with a face-centered cubic unit cell. The assemblies resembled natural viral inclusion bodies, and provide means for studying their self-assembly processes. In publication IV rod-like cellulose nanocrystals (CNC) were grafted with a cationic polymer. The cationic CNCs efficiently assembled the anionic icosahedral viruses. Additionally, the CNCs enabled the concentration and extraction of the viruses from solution. The assemblies can be further transferred to biomedical applications and allow the recovery of viruses via electrolyte-gated release. In publication V the CNCs were functionalized with cross-linkable alkyl chains and used for the reinforcement of a synthetic rubber. The moisture-repellent composites showed a hierarchical structure, where the CNCs assembled into ordered biomimetic structures at high weight fractions. Simultaneously the stress-strain behavior abruptly changed from nonlinear rubbery to almost linear with increasing CNC fraction, while the tensile modulus increased by almost two orders of magnitude.

KW - biohybrid material

KW - assembly

KW - DNA

KW - virus

KW - cellulose nanocrystal

KW - dendron

KW - dendrimer

KW - composite

KW - biohybridimateriaali

KW - virus

KW - nanokiteinen selluloosa

KW - dendroni

KW - dendrimeeri

KW - komposiitti

KW - biohybrid material

KW - assembly

KW - DNA

KW - virus

KW - cellulose nanocrystal

KW - dendron

KW - dendrimer

KW - composite

M3 - Doctoral Thesis

SN - 978-952-60-5971-6

T3 - Aalto University publication series DOCTORAL DISSERTATIONS

PB - Aalto University

ER -

Investigations of Bio-Organic Hybrid Assemblies

Abstrakti

Tutkimusalat

Pääsy asiakirjaan

Sormenjälki

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